CN102745782B - Electrodeionization method and electrodeionization apparatus for treating low concentration ionic solution - Google Patents
Electrodeionization method and electrodeionization apparatus for treating low concentration ionic solution Download PDFInfo
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- CN102745782B CN102745782B CN2012102061477A CN201210206147A CN102745782B CN 102745782 B CN102745782 B CN 102745782B CN 2012102061477 A CN2012102061477 A CN 2012102061477A CN 201210206147 A CN201210206147 A CN 201210206147A CN 102745782 B CN102745782 B CN 102745782B
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- Y02A20/124—Water desalination
Abstract
The invention discloses an electrodeionization method and an electrodeionization apparatus for treating a low concentration ionic solution, and relates to the technology of desalination and ultrapure water treatment. Adhering a material capable of catalyzing water dissociation (5) to one side facing to a light chamber of a cation exchange membrane (3) of the electrodeionization apparatus. A conversion degree of a resin in the light chamber can be easily controlled by changing the adhering positions of the catalytic layer (5) of the cation exchange membrane (3), changing types of the catalytic materials and changing resin filling ratios of a bed layer of the light chamber, and then a removal degree of salt ions can be controlled. With the abovementioned way, relatively high resin regeneration degree can be realized in a relatively low applied voltage, so that a relatively high ion removal rate can be realized at a relatively low operating voltage. The electrodeionization apparatus can significantly reduce the applied voltage and energy consumption, thus reducing an operating cost, so the electrodeionization apparatus has important application value in the field of heavy metal ion removement and ultrapure water production.
Description
Technical field
The present invention relates to a kind of method and device of processing the electrodeionization of lower concentration solion, for improvement of the electrodeionization system performance, relate in particular be attached with the water decomposition catalyzer on the light indoor cationic exchange membrane of electrodeionization, improve ion exchange resin regeneration degree in the bed of light chamber, to reduce membrane stack voltage and energy consumption, obtain higher ion remaval rate under lower energy consumption.
Background technology
In the ultrapure water preparation field, technology just progressively replaces traditional ion exchange method to electrodeionization (be called for short EDI) becomes the technology main flow.EDI is filled in ion exchange resin in the freshwater room of electrodialyzer, and ion-exchange is combined with electrodialysis, realizes the NEW TYPE OF COMPOSITE sepn process of electricity regeneration continuously of lower concentration ion deep removal and resin simultaneously.Relative electrodialytic technique, the increase of the resistance that the ion exchange resin of the light indoor filling of EDI has avoided low concentration solution to bring; Relative ion exchange technique, in the light chamber of EDI, the water decomposition of face has produced H
+and OH
-, this makes light chamber intermediate ion exchange resin be regenerated, and without consuming extra soda acid, carrys out regenerating ion exchange resin.The electrodeionization assembly comprises membrane stack, electrode and gripping unit, and wherein membrane stack is core component, and by several films, to forming, each film is to containing dense chamber dividing plate, cationic exchange membrane, light chamber dividing plate and anion-exchange membrane.Electromigration occurs in light indoor ion under the effect of electric field, and positively charged ion moves to cationic exchange membrane, and negatively charged ion moves to anion-exchange membrane.Zwitterion enters dense chamber through ion-exchange membrane under the effect of electric field, reaches thus the deionization purpose, and what exit, light chamber obtained is fresh water, and what exit, dense chamber obtained is dense water.
The transmission that anion-cation exchange resin in light chamber is zwitterion provides the passage of a high conductivity.In light chamber entrance location, former water conductivity is higher, and near the resin of salt type import has played the effect of transmitting salt ion; In outlet position, light chamber, the electrical conductivity of water after processing is reduced to 1/5-1/20 times of former water, and the resin of salt type can't transmit the salt ion that concentration is extremely low, the resin that this need to regenerate.The same with electrodialysis, light indoor anion and cation exchange membrane surface can form concentration polarization.When concentration polarization acquires a certain degree, water decomposition can occur in anion and cation exchange membrane and ion exchange resin surface.Water decomposition product H
+and OH
-under electric field, electromigration occurring, makes the resin regeneration of salt type.The resin of exit regeneration can make salt ion enter the resin-phase transmission, thereby increases the salt ion clearance, so water decomposition is the deionized prerequisite of the EDI degree of depth, but the existence of water decomposition can make again current efficiency reduce, water decomposition product H
+and OH
-moved the part electric current, this part electric current is unnecessary.This has just demonstrated the positive and passive effect of water decomposition in EDI, EDI need to produce more water decomposition and realize degree of depth deionization with regenerating ion exchange resin under higher concentration polarization, this makes EDI to work under high membrane stack voltage, and this has caused EDI could realize the deionized purpose of the degree of depth under higher membrane stack voltage.Therefore a current main problem of EDI is how under lower membrane stack voltage, to obtain higher clearance.
Some trials have been carried out, Chinese patent 200780019555.9 discloses a kind of technological method and device, disclosed the deviation that changes export and import position current density by the access resistance element, the method increases the outlet resistance of light chamber, make current offset arrive the import of light chamber, thereby make the electromigration under electric field of the more salt ion of entry zone pass out light chamber.But have following problem: the increase that (1) additional resistance element is covert undoubtedly the membrane stack total electrical resistance, reaching under same ion remaval rate, membrane stack voltage increases, energy consumption increases; (2) resistance added in exit is actually the function that realizes resistance by the bang path of obstruction ion, therefore when realizing current offset, increased the resistance of ion transport, thereby the salt ion in solution need be walked around resistance element and passes out light chamber when transmitting.In a word, this patent changes the electric current distribution of bed import to outlet by the measure of external resistor, played the effect of certain drift current, but the negative impact that the method is brought is comparatively outstanding, the external resistor element can make the total electrical resistance of electric deionizer increase, energy consumption increases the increase that will offset the ion remaval rate, and the existence of external resistor element has simultaneously hindered the bang path of ion, also makes the clearance of ion reduce.
U.S. Patent No. 6,284,124 and 6, the device thinking of 514,398 device and Chinese patent No.200780019555.9 is similar, and improvements are: in the ion exchange resin bed floor of light chamber, add nonconducting doping particle, the doping particle will reduce the resin bed local conductivity, thereby optimize resistance and the distribution of conductivity of import to the outlet resin bed, to change the ununiformity of current density, to improve the ion remaval rate of whole bed.But the problem that the method exists total electrical resistance to increase equally, simultaneously, do not provide the ion mass transfer channel in the particle of doping, hindered the mass transfer of ion, the problem that this two aspect brings energy consumption to increase equally.
Summary of the invention
Need under high membrane stack voltage, obtain the technological deficiency of higher ion remaval rate in order to overcome existing lower concentration solion (salt ion, heavy metal and metalloid ion) electrodeionization processing, the object of the present invention is to provide a kind of method of processing the electrodeionization of lower concentration solion, reliably, obtain than the electrodeionization of macroion clearance (EDI) efficiently under lower current densities.
Another object of the present invention is to provide a kind of device of processing the electrodeionization of lower concentration solion, change the resin regeneration rate by the face water decomposition severe degree that changes the light chamber of EDI ion-exchange membrane, thereby realize than the macroion clearance under lower membrane stack voltage.
A kind of device of processing the electrodeionization of lower concentration solion, that two groups of anion and cation exchange membrane groups are set between anode and negative electrode, every group of anion and cation exchange membrane group is comprised of the anion-exchange membrane and the cationic exchange membrane that are oppositely arranged, form dense chamber between two groups of adjacent anion and cation exchange membrane groups, form light chamber between every group of anion and cation exchange membrane group, two groups of anion and cation exchange membrane groups form respectively the first light chamber and the second light chamber, the light indoor anion-cation exchange resin bed that all is filled with, it is characterized in that having the water decomposition catalyst layer towards a side of light chamber on cationic exchange membrane.
The effect of the catalyzer adhered on cationic exchange membrane is that the water decomposition to face carries out catalysis, accelerates the water decomposition reaction, increases the generation of hydrogen ion and hydroxide ion, realizes producing the water decomposition of higher degree under lower membrane stack voltage.The water decomposition product makes the resin bed regeneration level improve, and this makes the ion remaval degree increase.Can change the speed that local face water decomposition reacts by attachment position and the area that changes catalyzer, can change the distribution that the face water decomposition reacts by filling proportion and the filling mode that changes the bed anion-cation exchange resin, can be easy to control the rate distribution of water decomposition reaction in the bed of light chamber, and then the regeneration level of control bed resin, thereby control the ion remaval degree.
A kind of method of processing the electrodeionization of lower concentration solion:
The water that contains salt ion is from the import input of the first light chamber bed of anion and cation exchange membrane formation, and vertical current is exported from outlet behind two first, second light chambers of mutually connecting;
Apply the electric field perpendicular to flow direction in light chamber, under electric field action, the salt ion in water is mass transfer between the anion-cation exchange resin that forms light chamber, and enters light chamber through ion-exchange membrane, realizes ion isolation;
In the bed import of light chamber, salt ion is mass transfer in the ion exchange resin of salt type, and in bed outlet position, light chamber, and the concentration of salt ion is far below entrance location, salt ion need to be in the resin of regeneration mass transfer.
Water decomposition catalyst layer described above can be any of chromium hydroxide and nickel hydroxide, is preferably nickel hydroxide.
Water decomposition catalyst layer described above only is distributed in the scope of the 40%-100% that approaches outlet on the cationic exchange membrane of the second light chamber, and the first light indoor Zeo-karb proportion is 40-70%; In the bed zone of the second light indoor attached catalyst, the Zeo-karb proportion is 30-60%, and in attached catalyst bed zone, the Zeo-karb proportion is not 50-60%;
Perhaps the water decomposition catalyst layer is distributed in the scope of the 20%-40% that approaches outlet on the cationic exchange membrane of the first and second light chambers simultaneously, the ratio of the Zeo-karb of filling in the bed of attached catalyst is 20%-40%, and other its ratios of zone are 45%-60%.
One side at Zeo-karb towards light chamber applies the water decomposition catalytic specie, makes face water decomposition speed of reaction increase, concentration polarization condition under lower membrane stack voltage and, and the face of anion and cation exchange membrane also can produce more OH by water decomposition
-and H
+, OH
-and H
+under the effect of electric field, electromigration enters light chamber, makes anion-cation exchange resin regenerate, thereby makes the resin bed regeneration level increase.Here it is makes more salt ions enter the resin-phase mass transfer of high conductivity, enters dense chamber through ion-exchange membrane and realizes separating.
The invention has the beneficial effects as follows:
In the ingress of light chamber bed, the resin bed of salt type provides a high conductivity passage for the lower concentration ion; In the exit of light chamber bed, the effect of salt type resin bed is less, and the mass transfer that the resin that needs regeneration is salt ion provides passage.Higher membrane stack voltage makes light chamber face produce violent concentration polarization, and violent concentration polarization makes face produce water decomposition.Owing to adhering to one deck catalyzer on cationic exchange membrane, the existence of water decomposition catalyzer makes under lower membrane stack voltage, and the face of cationic exchange membrane also can produce more OH by water decomposition
-, OH
-under the effect of electric field, electromigration enters light chamber, makes anionite-exchange resin regenerate.Due to anion-exchange membrane itself exist can catalytic hydrolysis from group, cationic exchange membrane and anion-exchange membrane water decomposition simultaneously produce respectively OH
-and H
+make anion-cation exchange resin regeneration, the increase of resin regeneration rate, make the zwitterion clearance also increase.
In the present invention, on cationic exchange membrane, the effect of water decomposition Catalytic Layer is to make the anode membrane face under low membrane stack voltage and weak concentration polarization condition, and a large amount of water decomposition reactions occurs.Cationic exchange membrane and anion-exchange membrane water decomposition simultaneously produce respectively OH
-and H
+make yin and yang resin regeneration, the increase of resin regeneration rate makes the zwitterion clearance also increase, and reduces membrane stack voltage when reaching the object removal rate, reduces energy consumption simultaneously, reduces processing cost.
The water decomposition catalyzer that the present invention adopts is heavy metal hydroxide, it is with low cost, easily obtain, catalyzer is better in cationic exchange membrane surface attachment performance, operation through hundreds of hours, the cationic exchange membrane surface catalyst is without coming off without dissolving, and the stability of catalyst layer is better, is applicable to long-time running.
The accompanying drawing explanation
Fig. 1 is two sections electric deionizer schematic diagram of one-level of the present invention program.
Fig. 2 is the structural representation of one section electric deionizer of one-level of the present invention program.
Fig. 3 means that cationic exchange membrane is attached with the light chamber partial enlarged drawing of catalyzer.
In figure: 1. anode; 2. negative electrode; 3. cationic exchange membrane; 4. anion-exchange membrane; 5. catalyst layer; 6. the first light chamber; 7. the second light chamber; 8. dense chamber; 9. Zeo-karb; 10. anionite-exchange resin; 11. utmost point chamber; 12. light chamber inlet; 13. light chamber outlet.
Embodiment
Below in conjunction with accompanying drawing, preferred embodiment of the present invention is described in detail, thereby so that advantages and features of the invention can be easier to be it will be appreciated by those skilled in the art that, protection scope of the present invention is made to more explicit defining.Yet should be understood to not limit the scope of the invention here, have benefited from the technician of the present invention's design, any change that inventive features described herein is made and further improvement, and other application that the present invention described herein is conceived, all belong to the scope of the invention.
Fig. 1 is two sections electric deionizer schematic diagram of one-level of the present invention program.As shown in Figure 1, that two groups of anion and cation exchange membrane groups are set between anode 1 and negative electrode 2, every group of anion and cation exchange membrane group is comprised of the anion-exchange membrane and the cationic exchange membrane that are oppositely arranged, form dense chamber 8 between two groups of adjacent anion and cation exchange membrane groups, form light chamber between every group of anion and cation exchange membrane group.Wherein, close on the interior first light chamber 6 that forms of one group of anion and cation exchange membrane group of negative electrode 2, close on the interior second light chamber 7 that forms of one group of anion and cation exchange membrane group of anode 1.Be filled with the ion exchange resin bed floor in the first light chamber 6 and the second light chamber 7, the filling proportion of anion-cation exchange resin is: the first interior Zeo-karb proportion in light chamber 6 is 40-70%; In the bed zone of the second light chamber 7 interior attached catalysts, the Zeo-karb proportion is 30-60%, and in attached catalyst bed zone, the Zeo-karb proportion is not 50-60%.Former water is from entrance 12 input of the first light chamber 6, from cross the first light chamber 6 from upper vertical current, then from the light chamber 7 of top inflow second, then from the outlet 13 of the second light chamber 7, flow out.Form series relationship between the first light chamber 6 and the second light chamber 7.Adhere to the water decomposition catalyzer in the scope of the 40%-100% of approaching outlet on the cationic exchange membrane 3 of the second light chamber 7, the cationic exchange membrane 3 of the first light chamber 6 is kept intact.
Fig. 2 is the structural representation of one section electric deionizer of one-level of the present invention program.
As shown in Figure 2, be on the cationic exchange membrane of the first light chamber 6 and the second light chamber 7 to approach in the scope of 20%-40% of outlet 13 with Fig. 1 difference and adhere to the water decomposition catalyzer.The first light chamber is consistent with the filling mode of the second light chamber, and the filling proportion of anion-cation exchange resin is: the ratio of the Zeo-karb of filling in the bed of attached catalyst is 20%-40%, and the ratio of other regional Zeo-karbs is 45%-60%.
When concentration polarization is strengthened to a certain degree, the face of anion-exchange membrane 4 itself contains the water decomposition catalytic group, make water decomposition accelerate, the catalyst that cationic exchange membrane 3 faces adhere to the face water decomposition, cationic exchange membrane 3 and anion-exchange membrane 4 produce water decomposition simultaneously.The water decomposition process as shown in Figure 3.The OH that the interfacial water of cationic exchange membrane 3 dissociates and produces
-enter light chamber under electromigration, the H that the water decomposition of anion-exchange membrane 4 produces
+enter light chamber under electromigration, make Zeo-karb 9 and anionite-exchange resin 10 regeneration simultaneously.Anion-cation exchange resin is regenerated simultaneously, makes the concentration of negative and positive salt ion reach degree of depth removal simultaneously, realizes being issued to the object removal rate at lower membrane stack voltage.
Embodiment 1
In this example, the EDI device is two sections of one-levels, as shown in Figure 1, two light chambers is arranged between electrode, a dense chamber, two utmost point chambers.Adopt the ruthenium dioxide electrode as anode, adopt stainless steel electrode as negative electrode.The size of He Ji chamber, dense chamber dividing plate is 100 * 400 * 2mm, and light chamber baffle dimensions is 100 * 400 * 5mm, and the film useful area is 250cm
2, adopt domestic homogeneous phase anion/cation exchange membrane.The catalyzer adhered in 60% of approaching outlet scope on cationic exchange membrane in the second light chamber 7 scopes is chromium hydroxide, on the cationic exchange membrane in the first light chamber 6 scopes, keeps intact.Adopt domestic polystyrene storng-acid cation exchange resin and strongly basic anion exchange resin, the resin particle diameter is 0.5mm.The filling proportion of anion-cation exchange resin is: the first interior Zeo-karb proportion in light chamber 6 is 70%; In the bed zone of the second light indoor attached catalyst, the Zeo-karb proportion is 35%, and other regional proportions are 60%.That enter He Nong chamber, light chamber is pre-configured CuSO
4former water, the cupric ion mass concentration is 50mg/L, pH is 6, dense chamber water cycle turnover electrodeionization system, utmost point chamber is the Na that mass concentration is 500gm/L
2sO
4solution.Raw water flow is 10L/h, and dense chamber circulating water flow is 2L/h, and utmost point chamber circulating water flow is 2L/h.
The power supply of direct current constant potential, the membrane stack operating voltage is 20V.Through the operation of 24 hours, the copper ion concentration of the light chamber of electrodeionization was lower than 0.08mg/L.After electrodeionization moves 500 hours, copper ion concentration is below 0.1mg/L.After 500 hours, use atomic force microscope to be observed the face catalyst layer, catalyzer adheres to degree of uniformity and initially basically identical.For illustrating that more clearly this example carries out, cationic exchange membrane is adhered to the electrodeionization system of catalytic specie and electrodeionization system that cationic exchange membrane does not have catalytic specie compares, in the identical situation of other conditions, cationic exchange membrane did not have the electric deionizer operation of attached water dissociation catalyst after 24 hours, and copper ion concentration is in the 0.22mg/L left and right.After operation 24 hours, if will reach the removal degree of same 0.08mg/L, need on the membrane stack operating voltage, be adjusted to the 32V left and right.
Embodiment 2
The device of embodiment 2, circulation process and operation steps etc. are substantially the same manner as Example 1, and difference from Example 1 is: the catalyzer adhered in 60% of approaching outlet scope on the cationic exchange membrane of the second light chamber is nickel hydroxide.Adopt domestic out-phase anion and cation exchange membrane.Through the operation of 24 hours, the water outlet copper ion concentration of the light chamber of electrodeionization was lower than 0.22mg/L.The electric deionizer operation is after 500 hours, and the removal ability is normal, without downtrending.After 500 hours, use atomic force microscope to be observed the face catalyst layer, catalyzer adheres to degree of uniformity with initial consistent.The effect of nickel hydroxide catalyzer slightly is worse than chromium hydroxide.
Device and the operation steps of embodiment 3 are substantially the same manner as Example 1, with the difference of embodiment 1, be: the EDI device is one section of one-level, as shown in Figure 2, raw water flow is 30L/h, and exporting in the first and second light chambers the catalyzer adhered on cationic exchange membrane in 35% length range is chromium hydroxide.In the first light chamber and the second light chamber, the filling proportion of anion-cation exchange resin is, the ratio of the Zeo-karb of filling in the attached catalyst zone is 30%, and other its ratios of zone are 60%.Through the operation of 24 hours, the water outlet copper ion concentration of the light chamber of electrodeionization was lower than 4.0mg/L.Through the long-time running of 500 hours, the removal ability of electrodeionization was normal, without downtrending.The electric deionizer operation is used atomic force microscope to be observed the face catalyst layer after 500 hours, catalyzer adheres to degree of uniformity with initial consistent.One section of one-level is suitable for hanging down the technique of removal degree.
The device of embodiment 4, circulation process and operation steps are substantially the same manner as Example 1, with the difference of embodiment 1, are: embodiment 4 is for the production of ultrapure water, and what enter He Nong chamber, light chamber is the pre-configured former water of NaCl, and specific conductivity is 50 μ s/cm.The filling proportion of anion-cation exchange resin is: the first light indoor Zeo-karb proportion is that 40%, the second light indoor catalyst area Zeo-karb proportion is 40%, and other regional proportions are 50%.The operation of spending 24 hours, the light chamber of electrodeionization goes out electrical conductivity of water lower than 0.12 μ s/cm.The electrodeionization operation is after 500 hours, and the removal ability is normal, without downtrending.After 500 hours, use atomic force microscope to be observed the face catalyst layer, catalyzer adheres to degree of uniformity with initial consistent.For illustrating that more clearly this example carries out, cationic exchange membrane is adhered to the electrodeionization system of catalytic specie and electrodeionization system that cationic exchange membrane does not have catalytic specie compares, in the identical situation of other conditions, cationic exchange membrane did not have the electric deionizer operation of attached water dissociation catalyst after 24 hours, and it is 0.26 μ s/cm that the light chamber of electrodeionization goes out electrical conductivity of water.After operation 24 hours, if will reach same removal degree, need to the 27V left and right will be adjusted on the membrane stack operating voltage.
The condition that embodiment 5 to embodiment 8 adopts is as shown in table 1
Table 1
The foregoing is only embodiments of the invention; not thereby limit the scope of the claims of the present invention; every equivalent structure or conversion of equivalent flow process that utilizes specification sheets of the present invention and accompanying drawing content to do; or directly or indirectly be used in other relevant technical fields, all in like manner be included in scope of patent protection of the present invention.
Claims (1)
1. the electric deionizer for the treatment of the lower concentration solion, that two groups of anion and cation exchange membrane groups are set between anode and negative electrode, every group of anion and cation exchange membrane group is comprised of the anion-exchange membrane and the cationic exchange membrane that are oppositely arranged, form dense chamber between two groups of adjacent anion and cation exchange membrane groups, form light chamber between every group of anion and cation exchange membrane group, two groups of anion and cation exchange membrane groups form respectively the first light chamber and the second light chamber, wherein the entrance containing ionized water is closed in the first light chamber, be close to the exit in the second light chamber, it is characterized in that the side towards the first light chamber and the second light chamber is attached with the water decomposition catalyst layer on cationic exchange membrane,
A kind of or the combination of the oxyhydroxide that the material of described water decomposition catalyst layer is heavy metal chromium and nickel;
Described water decomposition catalyst layer only is distributed in the scope of the 40%-100% that approaches outlet on the cationic exchange membrane of the second light chamber, and the first light indoor Zeo-karb proportion is 40-70%; In the bed zone of the second light indoor attached water dissociation catalyst layer, the Zeo-karb proportion is 30-60%, and in the bed zone of attached water dissociation catalyst layer, the Zeo-karb proportion is not 50-60%;
Perhaps the water decomposition catalyst layer is distributed in the scope of the 20%-40% that approaches outlet on the cationic exchange membrane of the first light chamber and the second light chamber simultaneously, the ratio of the Zeo-karb of filling in the bed of attached water dissociation catalyst layer is 20%-40%, and other regional Zeo-karb ratios are 45%-60%.
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| CN103102273B (en) * | 2012-12-29 | 2016-04-27 | 上海新阳半导体材料股份有限公司 | A kind of purification process of organic amine electroplating additive |
| CN106145465B (en) * | 2016-08-18 | 2019-05-21 | 东北大学 | Electrodeionization-electrodeposition process reuse cyanidation gold-extracted tail washings device and method |
| CN110092451A (en) * | 2018-01-27 | 2019-08-06 | 苏州斯贝孚光电科技有限公司 | A kind of Electroremediation adds the method for the integrated removal metal salt of permeating reaction wall system |
| WO2021166368A1 (en) * | 2020-02-18 | 2021-08-26 | 株式会社エフ・シー・シー | Ion exchange equipment |
| CN111233086A (en) * | 2020-03-16 | 2020-06-05 | 佛山市云米电器科技有限公司 | One-way anion exchange type water filtering and purifying system and method and water purifier |
| CN113929194B (en) * | 2020-06-29 | 2023-06-09 | 佛山市顺德区美的饮水机制造有限公司 | Water treatment device |
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|---|---|---|---|---|
| EP1386938A1 (en) * | 2001-04-13 | 2004-02-04 | Organo Corporation | Ion exchanger |
| US20100261921A1 (en) * | 2002-11-05 | 2010-10-14 | Lin Yupo J | Integrated System for the Production and Separation of Biodiesel and Method Thereof |
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| CF01 | Termination of patent right due to non-payment of annual fee |